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In most conceptual models of dissolution trapping of CO2, it is assumed that mixing of dissolved supercritical CO2 and formation brine occurs through density-driven convection. In our previous modeling study, we showed that the presence of continuous low-permeability shale layers in the formations causes convective shutdown through disruption of fingers, which impacts the effectiveness of mixing and trapping processes. However, these layers are naturally heterogeneous due to variations in compositional and textural properties. In the present study, we investigate the potential effects of heterogeneity present within semi-confining low-permeability layers on the overall mixing and trapping of dissolved CO2. Since accurate field experimentation in deep geologic formations is difficult due to inability to adequately characterize geology and define boundary conditions of the formation, we designed well-controlled experiments using NaBr solution and water under laboratory conditions. We conducted intermediate-scale 3D laboratory experiments under two homogeneous and one heterogeneous multilayered sand packing configurations. The results of these experiments show that connectivity of relatively higher permeability material within the semi-confining low-permeability layers contributes to mixing through (1) brine leakage between upper and lower aquifers (reverse convection), and (2) trapping through diffusion and back diffusion of initially trapped mass due to reversed concentration gradients in the long term. These findings suggest that when estimating the effectiveness of dissolution trapping in CO2 sequestration one needs to consider possible deviations from the traditional convective mixing theory in homogeneous media. Under some conditions of natural formation heterogeneity, diffusion can contribute to trapping; in some others, it may not.

Carbon Capture and Storage (CCS) represents a technology aimed to reduce atmospheric loading of CO2 from power plants and heavy industries by injecting it into deep geological formations, such as saline aquifers. A number of trapping mechanisms contribute to effective and secure storage of the injected CO2 in supercritical fluid phase (scCO2) in the formation over the long term. The primary trapping mechanisms are structural, residual, dissolution and mineralization. Knowledge gaps exist on how the heterogeneity of the formation manifested at all scales from the pore to the site scales affects trapping and parameterization of contributing mechanisms in models. An experimental and modeling study was conducted to fill these knowledge gaps. Experimental investigation of fundamental processes and mechanisms in field settings is not possible as it is not feasible to fully characterize the geologic heterogeneity at all relevant scales and gathering data on migration, trapping and dissolution of scCO2. Laboratory experiments using scCO2 under ambient conditions are also not feasible as it is technically challenging and cost prohibitive to develop large, two- or three-dimensional test systems with controlled high pressures to keep the scCO2 as a liquid. Hence, an innovative approach that used surrogate fluids in place of scCO2 andmore » formation brine in multi-scale, synthetic aquifers test systems ranging in scales from centimeter to meter scale developed used. New modeling algorithms were developed to capture the processes controlled by the formation heterogeneity, and they were tested using the data from the laboratory test systems. The results and findings are expected to contribute toward better conceptual models, future improvements to DOE numerical codes, more accurate assessment of storage capacities, and optimized placement strategies. This report presents the experimental and modeling methods and research results.« less